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Simultaneous observation of atmospheric peroxyacetyl nitrate and ozone in the megacity of Shanghai, China: Regional transport and thermal decomposition
2021
Zhang, Gen | Jing, Shengao | Xu, Wanyun | Gao, Yaqin | Yan, Chao | Liang, Linlin | Huang, Cheng | Wang, Hongli
Atmospheric peroxyacetyl nitrate (PAN) and ozone (O₃) are two typical indicators for photochemical pollution that have adverse effects on the ecosystem and human health. Observation networks for these pollutants have been expanding in developed regions of China, such as North China Plain (NCP) and Pearl River Delta (PRD), but are sparse in Yangtze River Delta (YRD), meaning their concentration and influencing factors remain poorly understood. Here, we performed a one-year measurement of atmospheric PAN, O₃, particulate matter with aerodynamic diameter smaller than 2.5 μm (PM₂.₅), nitrogen oxides (NOₓ), carbon monoxide (CO), and meteorological parameters from December 2016 to November 2017 in Shanghai. Overall, high hourly maximum PAN and O₃ were found to be 7.0 and 185 ppbv in summer, 6.2 and 146 ppbv in autumn, 5.8 and 137 ppbv in spring, and 6.0 and 76.7 ppbv in winter, respectively. Continental air masses probably carried atmospheric pollutants to the sampling site, while frequent maritime winds brought in less polluted air masses. Furthermore, positive correlations (R: 0.72–0.85) between PAN and O₃ were found in summer, indicating a predominant role of photochemistry in their formation. Unlike in summer, weak or no correlations between PAN and O₃ were featured during the other seasons, especially in winter, due to their different loss pathways. Unexpectedly, positive correlations between PAN and PM₂.₅ were found in all seasons. During summer, moderate correlation could be attributed to the strong photochemistry acting as a common driver in the formation of secondary aerosols and PAN. During winter, high PM₂.₅ might promote PAN production through HONO production, hence resulting in a good positive correlation. Additionally, the loss of PAN by thermal decomposition (TPAN) only accounted for a small fraction (ca. 1%) of the total (PAN + TPAN) during a typical winter episode, while it significantly reached 14.4 ppbv (71.1% of the total) in summer.
显示更多 [+] 显示较少 [-]Impact of residual layer transport on air pollution in Beijing, China
2021
Liu, Yusi | Tang, Guiqian | Wang, Meng | Liu, Baoxian | Hu, Bo | Chen, Qi | Wang, Yuesi
The residual layer (RL) stores a large amount of pollutants, but its effect on near-surface pollution is unknown. In this study, a two-year continuous observation was performed in Beijing using a ceilometer. The generalized boundary layer includes the mixing layer and RL. The results showed that there is no significant seasonal difference in the generalized boundary layer height (GBLH). The average GBLHs in spring, summer, autumn and winter are 1155, 1139, 1036 and 1195 m, respectively. The diurnal variation characteristics of spring, summer and autumn are similar, and the RL disappears when the mixing layer height reaches its peak in the afternoon. In winter, the development of the mixing layer is weak, and there is a 33.8% chance that the RL cannot be breached, thus making the mixing layer height at noon much lower than the GBLH. The concentrations of PM₂.₅ in the mixing layer and RL are 89 and 52 μg m⁻³, respectively, and the probability that the PM₂.₅ concentration in the RL was higher than that near the ground was 38.9%. RL transport represents an important beginning of the pollution event during the winter mornings and afternoons in Beijing. This study is helpful to better understand the structure of the RL and its influence on air pollution.
显示更多 [+] 显示较少 [-]Health and ecological risk assessment based on pesticide monitoring in Saïss plain (Morocco) groundwater
2021
Berni, Imane | Menouni, Aziza | El Ghazi, Ibrahim | Godderis, Lode | Duca, Radu-Corneliu | Jaafari, Samir El
In many countries, including Morocco, groundwater contamination with pesticides such as globally banned organochlorides (e.g., dichlorodiphenyltrichloroethane (DDT)) and some accredited organophosphates and pyrethroids poses ecological and human health risks. To assess these risks, we herein monitored pesticides in Saïss plain groundwater (Morocco) during the summer of 2017 and the winter of 2018 using polar organic chemical integrative samplers. The two types of passive samplers were deployed in 22 traditional wells for 14–20 days and subjected to solid-phase extraction. The extracts were analyzed by gas chromatography-mass spectrometry and liquid chromatography-tandem mass spectrometry using a multiresidue method, and 27 pesticides were detected in total. In the summer campaign, 22 pesticides with individual concentrations ranging from <limit of quantitation (LOQ) to 243.1 ng L⁻¹ were identified, whereas 17 compounds with concentrations ranging from <LOQ to 53.8 ng L⁻¹ were detected in the winter campaign. In the summer period, the maximum individual concentrations of chlorothalonil, DDT, and α-hexachlorocyclohexane (α-HCH) equaled 111.7, 36.1, and 22.3 ng L⁻¹, respectively, with the respective values for the winter period equaling 18.14, 16.62, and 22.2 ng L⁻¹. Health risk assessment indicated that the carcinogenic α-HCH, β-HCH, DDT, and dichlorodiphenyldichloroethylene present in groundwater may also contaminate drinking water and thus pose a threat to human health, particularly to that of infants and children. Further analysis revealed that the Saïss aquifer presents a high ecological risk. Thus, the monitoring of pesticides in groundwater by passive sampling was effective and could be combined with human health and ecological risk assessment to develop ways of reducing human and environmental exposure to pesticides.
显示更多 [+] 显示较少 [-]Heavy ozone pollution episodes in urban Beijing during the early summertime from 2014 to 2017: Implications for control strategy
2021
Zhang, Xin | Li, Hong | Wang, Xuezhong | Zhang, Yujie | Bi, Fang | Wu, Zhenhai | Liu, Yuhong | Zhang, Hao | Gao, Rui | Xue, Likun | Zhang, Qingzhu | Chen, Yizhen | Chai, Fahe | Wang, Wenxing
Ground-level ozone (O₃) has become the principal air pollutant in Beijing during recent summers. In this context, an investigation of ambient concentrations and variation characteristics of O₃ and its precursors in May and June from 2014 to 2017 in a typical urban area of Beijing was carried out, and the formation sensitivity and different causes of heavy O₃ pollution (HOP, daily maximum 8-h O₃ (MDA8h O₃)>124 ppbv) were analyzed. The results showed that the monthly assessment values of the O₃ concentrations (the 90ᵗʰ percentile MDA8h O₃ within one month) were highest in May or June from 2014 to 2017, and the values presented an overall increasing trend. During this period, the number of O₃ pollution days (MDA8h O₃ > 75 ppbv) also showed an increasing trend. During the HOP episodes, the concentrations of volatile organic compounds (VOCs), nitrogen oxides (NOX), and carbon monoxide (CO) were higher than their respective mean values in May and June, and the meteorological conditions were more conducive to atmospheric photochemical reactions. The HOP episodes were mainly caused by local photochemical formation. From 2014 to 2017, O₃ formation during the HOP episodes shifted from VOC and NOX mixed-limited to VOC-limited conditions, and O₃ formation was most sensitive to anthropogenic VOCs. Six categories of VOC sources were identified, among which vehicular exhaust contributed the most to anthropogenic VOCs. The VOC concentrations and OFPs of anthropogenic sources have decreased significantly in recent years, indicating that VOC control measures have been effective in Beijing. Nevertheless, NOX concentrations did not show an evident decreasing trend in the same period. Therefore, more attention should be devoted to O₃ pollution control in May and June; control measure adjustments are needed according to the changes in O₃ precursors, and coordinated control of VOCs and NOX should be strengthened in long-term planning.
显示更多 [+] 显示较少 [-]Environmental and health risks of VOCs in the longest inner–city tunnel in Xi’an, Northwest China: Implication of impact from new energy vehicles
2021
Xu, Hongmei | Feng, Rong | Wang, Zexuan | Zhang, Ningning | Zhang, Renjian | He, Kailai | Wang, Qiyuan | Zhang, Qian | Sun, Jian | Zhang, Bin | Shen, Zhenxing | Ho, Steven Hang Sai | Cao, Junji
Traffic source–dominated volatile organic compound (VOC) samples were collected during four time-intervals in a day (Ⅰ: 7:30–10:30, Ⅱ: 11:00–14:00, Ⅲ: 16:30–19:30, and Ⅳ: 20:00–23:00) in a tunnel in summer, 2019, in Xi’an, China. The total measured VOC (TVOC) in periods Ⅰ and Ⅲ (rush hours, 107.2 ± 8.2 parts per billion by volume [ppbv]) was 1.8 times that in periods Ⅱ and Ⅳ (non-rush hours, 58.6 ± 13.8 ppbv), consistent with the variation in vehicle numbers in the tunnel. The considerably elevated ethane and ethylbenzene levels could have been attributed to emissions from compressed natural gas vehicles and the rapid development of methanol-fueled taxis in Xi’an in 2019. The mixing ratios of benzene, toluene, ethylbenzene, and xylenes (BTEX) contributed 9.4%–12.7% to TVOCs, and the contributions were nearly 40% higher in periods Ⅰ and Ⅲ than in Ⅱ and Ⅳ, indicating that BTEX levels were strongly affected by vehicle emissions. The indicators of motor vehicle emission, namely ethylene, propylene, toluene, m/p-xylenes, o-xylene, and propane, contributed to more than half of the ozone formation potential in this study. The noncarcinogenic risks of VOCs in this study were within the international safety standard, whereas the carcinogenic risks exceeded the standard by 2.3–4.6 times, suggesting that carcinogenic risks were more serious than noncarcinogenic risks. VOCs presented 2.2 and 1.4 times noncarcinogenic and carcinogenic risks during rush hours than during non-rush hours, respectively. Notably, the carcinogenic risk in period Ⅳ was comparable with that in period Ⅲ; however, the vehicle numbers and VOC mixing ratios were the lowest at night, which may have attributed to the increasing number and proportion of methanol M100-fueled vehicles in the tunnel. Therefore, VOCs emitted by new energy vehicles should also be seriously considered while evaluating fossil fuel vehicle emissions.
显示更多 [+] 显示较少 [-]Understanding the spatiotemporal pollution dynamics of highly fragile montane watersheds of Kashmir Himalaya, India
2021
Bhat, Sami Ullah | Khanday, Shabir A. | Islam, Sheikh Tajamul | Sabha, Inam
Pollution of riverine ecosystems through the multidimensional impact of human footprints around the world poses a serious challenge. Research studies that communicate potential repercussions of landscape structure metrics on snowmelt riverine water quality particularly, in climatically fragile Himalayan watersheds are very scarce. Though, worldwide, grasping the influence of land-use practices on water quality (WQ) has received renewed attention yet, the relevance of spatial scale linked to landscape pattern is still elusive due to its heterogenic nature across diverse geomorphic regions. In this work, therefore, we tried to capture the insights on landscape-aquascape interface by juxtapositioning the impacts of landscape structure pattern on snowmelt stream WQ of the whole Jhelum River Basin (JRB) under three varying spatial scales viz., watershed scale, riparian corridor (1000 m wide) and reach buffer (500 m wide). The percentage of landscape pattern composition and configuration metrics in the JRB were computed in GIS utilizing Landsat-8 OLI/TIRS satellite image having 30 m resolution. To better explicate the influence of land-use metrics on riverine WQ with space and time, we used Redundancy analysis (RDA) and multilinear regression (MLR) modeling. MLR selected land-use structure metrics revealed the varied response of WQ parameters to multi-scale factors except for total faecal coliform bacteria (TC) which showed perpetual presence. The reach-scale explained slightly better (76%) variations in WQ than riparian (75%) and watershed (70%) scales. Likewise, across seasonal scale, autumn (75%), winter (83%), and summer (77%) captured the most WQ variation at catchment, riparian, and reach scales respectively. We observed impairing WQ linkages with agriculture, built-up and barren rocky areas across watersheds, besides, pastures in riparian buffer areas, and fragmentation of landscape patches at the reach scale. Due to little appearance of spatial scale differences, a multi scale perspective landscape planning is emphasized to ensure future sustainability of Kashmir Himalayan water resources.
显示更多 [+] 显示较少 [-]Optical properties and 14C ages of stream DOM from agricultural and forest watersheds during storms
2021
Lee, Seung-Cheol | Shin, Yera | Jeon, Young-Joon | Lee, Eun-Ju | Eom, Jae-Sung | Kim, Bomchul | Oh, Neung-Hwan
Forest and agricultural land use affects the concentration and composition of dissolved organic carbon (DOC) in streams and rivers. To elucidate the impacts of forest and agricultural land use on stream DOC during storm events, we investigated DOC concentration ([DOC]), optical properties of dissolved organic matter (DOM), and Δ¹⁴C-DOC in both forest- and agriculture-dominated headwater streams in South Korea in the summer of 2012. One forested and five agricultural streams were investigated. During storms, the peak [DOC] of forest stream increased to 5.8 mg L⁻¹, approximately two times larger than that of the most agricultural stream (3.2 mg L⁻¹), demonstrating the weaker storm responses of the [DOC] of agricultural streams to hydrological change. Five PARAFAC components were identified, including three terrestrial humic-like substances (C1, C2, C3), one microbial humic substance (C4), and one microbial protein-like substances (C5). The mean (C4+C5)/(C1+C2+C3) of all storm events at the most agricultural stream was 1.5 times larger than that of the most forested stream, suggesting that more protein-like DOM is exported from agricultural watersheds. Whereas a forest stream was primarily composed of terrestrially derived and ¹⁴C-enriched modern DOC, the ¹⁴C-age of the most agricultural stream was up to ∼1000 years old. The results suggest that agricultural practices could decrease the old organic carbon pools from soils. However, how quickly the aged DOC can be degraded to CO₂ in streams is unknown, warranting future investigation on lability of the aged DOC and their effects on CO₂ evasion from rivers and estuaries downstream.
显示更多 [+] 显示较少 [-]Transboundary transport of ozone pollution to a US border region: A case study of Yuma
2021
Qu, Zhen | Wu, Dien | Henze, Daven K. | Li, Yi | Sonenberg, Mike | Mao, Feng
High concentrations of ground-level ozone affect human health, plants, and animals. Reducing ozone pollution in rural regions, where local emissions are already low, poses challenge. We use meteorological back-trajectories, air quality model sensitivity analysis, and satellite remote sensing data to investigate the ozone sources in Yuma, Arizona and find strong international influences from Northern Mexico on 12 out of 16 ozone exceedance days. We find that such exceedances could not be mitigated by reducing emissions in Arizona; complete removal of state emissions would reduce the maximum daily 8-h average (MDA8) ozone in Yuma by only 0.7% on exceeding days. In contrast, emissions in Mexico are estimated to contribute to 11% of the ozone during these exceedances, and their reduction would reduce MDA8 ozone in Yuma to below the standard. Using satellite-based remote sensing measurements, we find that emissions of nitrogen oxides (NOₓ, a key photochemical precursor of ozone) increase slightly in Mexico from 2005 to 2016, opposite to decreases shown in the bottom-up inventory. In comparison, a decrease of NOₓ emissions in the US and meteorological factors lead to an overall of summer mean and annual MDA8 ozone in Yuma (by ∼1–4% and ∼3%, respectively). Analysis of meteorological back-trajectories also shows similar transboundary transport of ozone at the US-Mexico border in California and New Mexico, where strong influences from Northern Mexico coincide with 11 out of 17 and 6 out of 8 ozone exceedances. 2020 is the final year of the U.S.-Mexico Border 2020 Program, which aimed to reduce pollution at border regions of the US and Mexico. Our results indicate the importance of sustaining a substantial cooperative program to improve air quality at the border area.
显示更多 [+] 显示较少 [-]Vertical profile of aerosols in the Himalayas revealed by lidar: New insights into their seasonal/diurnal patterns, sources, and transport
2021
Xiang, Yan | Zhang, Tianshu | Liu, Jianguo | Wan, Xin | Loewen, Mark | Chen, Xintong | Kang, Shichang | Fu, Yibin | Lv, Lihui | Liu, Wenqing | Cong, Zhiyuan
Atmospheric aerosols play a crucial role in climate change, especially in the Himalayas and Tibetan Plateau. Here, we present the seasonal and diurnal characteristics of aerosol vertical profiles measured using a Mie lidar, along with surface black carbon (BC) measurements, at Mt. Qomolangma (QOMS), in the central Himalayas, in 2018–2019. Lidar-retrieved profiles of aerosols showed a distinct seasonal pattern of aerosol loading (aerosol extinction coefficient, AEC), with a maximum in the pre-monsoon (19.8 ± 22.7 Mm⁻¹ of AEC) and minimum in the summer monsoon (7.0 ± 11.2 Mm⁻¹ of AEC) seasons. The diurnal variation characteristics of AEC and BC were quite different in the non-monsoon seasons with enriched aerosols being maintained from 00:00 to 10:00 in the pre-monsoon season. The major aerosol types at QOMS were identified as background, pollution, and dust aerosols, especially during the pre-monsoon season. The occurrence of pollution events influenced the vertical distribution, seasonal/diurnal patterns, and types of aerosols. Source contribution of BC based on the weather research and forecasting chemical model showed that approximately 64.2% ± 17.0% of BC at the QOMS originated from India and Nepal in South Asia during the non-monsoon seasons, whereas approximately 47.7% was from local emission sources in monsoon season. In particular, the high abundance of BC at the QOMS in the pre-monsoon season was attributed to biomass burning, whereas anthropogenic emissions were the likely sources during the other seasons. The maximum aerosol concentration appeared in the near-surface layer (approximately 4.3 km ASL), and high concentrations of transported aerosols were mainly found at 4.98, 4.58, 4.74, and 4.88 km ASL in the pre-monsoon, monsoon, post-monsoon, and winter seasons, respectively. The investigation of the vertical profiles of aerosols at the QOMS can help verify the representation of aerosols in the air quality model and satellite products and regulate the anthropogenic disturbance over the Tibetan Plateau.
显示更多 [+] 显示较少 [-]The diurnal cycle of summer tropospheric ozone concentrations across Chinese cities: Spatial patterns and main drivers
2021
Xia, Nan | Du, Enzai | Guo, Zhaodi | de Vries, Wim
China is experiencing severe tropospheric ozone pollution, especially during the summer period in cities. Previous studies have assessed the role of meteorological conditions and anthropogenic precursors in shaping the diurnal variation of ozone concentration in some Chinese cities or the spatial patterns of daytime ozone concentration, but less is known about the spatial variation and main regulators of the diurnal cycle of summer ozone concentrations in Chinese cities. Using monitoring data from 367 cities, we analyzed the spatial patterns and main regulators of daytime maximum, nighttime minimum and diurnal difference of summer (June–August) ozone concentration during 2015–2019. National mean values and standard deviations of daytime maximum and nighttime minimum of summer surface ozone concentration were 124.1 ± 27.5 and 33.4 ± 13.0 μg m⁻³, resulting in a diurnal difference of 90.7 ± 25.2 μg m⁻³. High values of daytime maximum, nighttime minimum, and diurnal difference of summer ozone concentration occurred in cities in northern China, especially in the North China Plain, and several city agglomerations in southern China. Daytime maximum ozone concentration was higher in cities with higher daytime PM₂.₅ and NO₂ concentrations, lower daytime precipitation and lower elevation. Nighttime minimum ozone concentration increased with lower nighttime precipitation, lower NO₂ concentration and CO concentration, higher nighttime maximum PM₂.₅ concentration and higher elevation. Diurnal difference of ozone concentration increased with lower elevation, lower daytime precipitation, and higher diurnal difference of CO and NO₂ concentrations. Our findings highlight different regulators for daytime and nighttime ozone and imply the need of joint regulation of PM₂.₅ and NO₂ emissions to control ozone pollution.
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